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At least 91 records · Page 5

Atomic-scale tuned interface of nickel-rich cathode for enhanced electrochemical performance in lithium-ion batteries

The Ni-rich layered LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC6 22 ) is one promising cathode for lithium-ion batteries (LIBs), but suffers from poor cycling stability under high cutoff potentials. The performance degradation was reflected as capacity fading and voltage drop, having their roots in instable interface of NMC622. Aimed at improving interfacial stability, in this study, we deposited nanoscale ZrO 2 coatings conformally over NMC622 cathodes using atomic layer deposition (ALD). We found that, under a high cutoff voltage (4.5 V), the ALD ZrO 2 coatings evidently improved the performance of NMC622 cathode, showing better cyclability and higher sustainable capacity. In addition, the ALD coatings dramatically boosted the rate capability of NMC622. All these compelling performance results are ascribed to the atomic-scale tunable ZrO 2 coatings via ALD, which create stable interface and thereby inhibit unfavorable evolutions. In the study, we utilize a suite of characterization tools and various analyses to clarify the effects of ALD ZrO 2 coatings. This study will be helpful for improving the performance of nickel-rich cathodes via interfacial engineering using ALD.

25 ENERGY STORAGE↗

Wet chemical synthesis and properties of argyrodite sulfide solid electrolytes for solid state lithium batteries

The commercialization of the lithium-ion battery (LIB) in 1991 was responsible for the explosion in portable electronic technologies that has been seen over the past 30 years. With the advent of electric vehicles and other high-powered technologies, there is tremendous demand for LIBs with higher energy density and high safety. To achieve this, new electrode materials must be explored. The obvious choice of anode material would be pure metal lithium, which has a theoretical specific capacity of 3860 mAh g-1 . Unfortunately, metal lithium anodes have not been widely commercialized due to their tendency to react violently with the flammable liquid electrolytes used in today’s batteries. Battery safety can best be achieved by adopting solid electrolytes in place of liquid electrolytes. Solid electrolytes are nonvolatile and nonflammable, safely allowing for the combination of high-capacity cathode materials with a Li metal anode. Argyrodite sulfide solid electrolytes such as halogen-doped Li6PS5X (X = Cl, Br, I) are noted for their high ionic conductivity. But before sulfides can be commercially adopted, they possess several disadvantages which must be addressed, including time- and energy-consuming synthesis processes, poor electrochemical stability, and intrinsically poor air stability. This dissertation seeks to address each of these challenges through materials design an synthesis strategies. In this work, we pioneer a solvent-based approach for the synthesis of argyrodite solid electrolytes Li7PS6 and Li6PS5Xinstead of a stringent solid-state synthesis. Nontoxic ethanol is employed as the solvent, enabling a rapid synthetic approach to produce argyrodite solid electrolytes with high phase purity and compositional flexibility. Compared with Li7PS6, halogen doping (i.e. X = F, Cl, Br, I) not only increases the ionic conductivity, but also enhances the electrochemical stability at the interface towards Li metal. Specifically, F-doped argyrodites produce a robust SEI layer containing LiF, contributing to enhanced interfacial stability. Finally, to address the air instability challenge, argyrodite-incorporated composite solid electrolytes (CSEs) are designed and prepared to produce stable and flexible membranes that are demonstrated in solid-state Li metal batteries. These advances push argyrodite sulfide solid electrolyte research further and pave the way for the proliferation of next generation lithium metal batteries.

25 ENERGY STORAGE↗

Fluid dynamic mathematical aspects of supernova remnants

Supernovae—explosions of stars—are a central problem in astrophysics since they contain information on the entire process of stellar evolution and nucleosynthesis. Rayleigh–Taylor (RT) and Richtmyer–Meshkov (RM) instabilities, developing during the supernova blast, lead to intense interfacial RT/RM mixing of the star's materials and couple astrophysical to atomic scales. This work analyzes some fluid dynamic mathematical aspects of the titanic task of supernova's blast. We handle mathematical challenges of RT/RM dynamics in supernova relevant conditions by directly linking the conservation laws governing RT/RM dynamics to symmetry-based momentum model, by exactly deriving the model parameters in the scale-dependent and scale-invariant regimes, and by exploring the special self-similar class for RT/RM interfacial mixing with variable accelerations. Here we reveal that RT/RM dynamics is strongly influenced by deterministic (the initial and the flow) conditions in the scale-dependent linear and nonlinear regimes and in the self-similar mixing regime. The theory outcomes are consistent with the observations of supernova remnants, explain the results of the scaled laboratory experiments in high energy density plasmas, and yield the design of future experiments for the accurate quantification of RT/RM dynamics in supernova relevant conditions. We find that from fluid dynamic mathematical perspectives, supernovae can be regarded as an astrophysical initial value problem. Along with the guidance of what explodes at microscopic scales, supernova remnants encapsulate information on the explosion hydrodynamics and the associated deterministic conditions at macroscopic scales. We urge such effects be considered in interpretations of the observational data.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Morphology selection in dealloying: A phase field study of the coupling among kinetic mechanisms

A phase field model is used to investigate how the corrosion rate and morphology of a dealloying metal is controlled by the kinetic rates of bulk solid diffusion, interfacial diffusivity, and interface dissolution. A specific focus is investigating the manner by which variations in these kinetic parameters synergistically influence the onset of a morphological instability at the solid-liquid interface, which is known to precede rapid dealloying corrosion towards highly topologically complex structures such as bicontinuous porous solids. This work demonstrates that this instability can be suppressed by either an increase of interdiffusion in the solid alloy, or by a decreasing rate of dissolution at the solid-liquid interface. When the instability is suppressed, the result is a relatively planar, passivated dealloying front. Importantly, however, coupled changes in kinetic parameters can also promote the morphological instability and sustain fine-scale ligament and pore formation. Finally, the relevance of the solid-liquid interfacial diffusion for determining the rate of dealloying and ligament formation is highlighted. By elucidating the mechanistic influence of bulk and interfacial kinetic factors on the dealloyed morphology, this work helps to rationalize the contrasting morphologies observed in various dealloying systems.

Diffusion↗

Interfacial Pressure Improves Calendar Aging of Lithium Metal Anodes

Lithium metal is a very attractive anode material because its theoretical specific capacity is approximately 10 times higher than conventional graphite anodes. Despite great promise, Li anodes suffer from capacity fade due to instabilities with the electrolyte as well as stranding of active Li. We have previously shown that applied interfacial pressure improves Li anode cycling because the pressure reduces the propensity for Li isolation and enables easier reconnection. Many researchers have also shown that calendar aging can lead to Li capacity loss and this has been attributed to either electrolyte decomposition with concurrent Li corrosion or to the formation of stranded Li. Our prior research focused on calendar aging during cycling suggests the mechanism for calendar aging is largely related to stranding of Li during rest and reconnection of the stranded Li upon further cycling, evidenced by similar average Coulombic efficiencies and Li loss in cells with and without rest. Because our calendar aging studies suggest Li stranding as a major cause of Coulombic efficiency drops and our Li cycling studies suggest this can be mitigated partially through applied interfacial pressure, we hypothesized that applied pressure would improve calendar aging by reducing stranded Li and enabling reconnection. We systematically varied applied pressure (0-1000 kPa) on Li metal anodes during cycling tests with and without intermittent calendar aging periods. Though the Coulombic efficiency decreases during aging periods, the lost capacity is recovered during subsequent cycles, as shown though average Coulombic efficiency and cumulative Li capacity loss analysis. We find that application of pressure partially mitigates calendar aging, in accordance with our hypothesis that calendar aging is caused by Li standing and can be mitigated to some degree with interfacial pressure. This is further supported by our results showing that the average Coulombic efficiency and cumulative Li capacity losses are similar over 50 cycles for cells that were continuously cycled and cells with periodic calendar aging periods. This result indicates that the losses during aging are reversible, which is consistent with Li stranding and reconnection. We show that pressure is one mitigation technique that helps reduce Li calendar aging in this study, but our finding that calendar aging is primarily governed by the stranding and reconnection of dead Li has wider implications. This research suggests that other mitigations which have been shown to prevent dead Li formation or encourage reconnection during cycling would also likely be successful for the purpose of improving calendar aging. The authors were supported by a Laboratory Directed Research and Development (LDRD) program. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC (NTESS), a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy's National Nuclear Security Administration (DOE/NNSA) under contract DE-NA0003525. This written work is authored by an employee of NTESS. The employee, not NTESS, owns the right, title and interest in and to the written work and is responsible for its contents. This work was authored in part by the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy, LLC, for the U.S. Department of Energy (DOE) under Contract No. DE-AC36-08GO28308. Any subjective views or opinions that might be expressed in the written work do not necessarily represent the views of the U.S. Government.

applied pressure↗

Metal Oxide-Induced Instability and Its Mitigation in Halide Perovskite Solar Cells

Halide perovskite solar cells (PSCs) have emerged as a promising photovoltaic technology for sustainable energy solutions due to their impressive power conversion efficiency and a path to be manufactured by low-cost, high-throughput methods. To reach PSCs’ full potential for practical implementation, it is crucial to solving the issues related to its long-term operational stability. Furthermore, given that PSCs consist of many layers of dissimilar materials which form multiple internal interfaces, it is prudent to examine whether there exist interfacial interactions, most importantly between transport layers and perovskite absorbers, that can trigger device performance and instability. In this perspective, we bring to the attention of the PSC research community the lesser-known interfacial degradation of halide perovskites promoted by contact with metal oxide transport layers and highlight the deleterious effects on the PSCs’ performance and stability. We also discuss various mitigation strategies that have shown promises to achieve high-performing and stable PSCs.

14 SOLAR ENERGY↗

Design principles of heterointerfacial redox chemistry for highly reversible lithium metal anode

High electrochemical reversibility is required for the application of high-energy-density lithium (Li) metal batteries; however, inactive Li formation and SEI (solid electrolyte interface)-instability-induced electrolyte consumption cause low Coulombic efficiency (CE). The prior interfacial chemical designs in terms of alloying kinetics have been used to enhance the CE of Li metal anode; however, the role of its redox chemistry at heterointerfaces remains a mystery. Herein, the relationship between heterointerfacial redox chemistry and electrochemical transformation reversibility is investigated. It is demonstrated that the lower redox potential at heterointerface contributes to higher CE, and this enhancement in CE is primarily due to the regulation of redox chemistry to Li deposition behavior rather than the formation of SEI films. Low oxidation potential facilitates the formation of the surface with the highly electrochemical binding feature after Li stripping, and low reduction potential can maintain binding ability well during subsequent Li plating, both of which homogenize Li deposition and thus optimize CE. In particular, Mg hetero-metal with ultra-low redox potential enables Li metal anode with significantly improved CE (99.6%) and stable cycle life for 700 cycles at 3.0 mA cm -2 . This work provides insight into the heterointerfacial design principle of next-generation negative electrodes for highly reversible metal batteries.

25 ENERGY STORAGE↗

Design of High-Voltage Stable Hybrid Electrolyte with an Ultrahigh Li Transference Number

Considering the high energy consumption during processing, and the low compliance and adhesion of ceramic electrolytes, the integration of polymer into ceramic electrolytes provides a way to mitigate the interfacial issues. However, the severe ion concentration gradient, low ionic conductivity, and instability toward Li metal and high-voltage cathodes become the major concerns in applying hybrid electrolytes. In this work, we report a single-ionconducting hybrid electrolyte (SIE-LLZO) with 64 wt % Li 7 La 3 Zr 2 O 12 (LLZO) particles embedded in a fluoroboron-centered Li-conductive polymer framework (LiBFSIE). The SIE-LLZO electrolyte exhibited a high Li transference number of 0.94 and electrochemical stability up to 5.6 V vs Li/Li + . Promising averaged Coulombic efficiencies of 99.97% and 99.91% were achieved in cells with LiNi 0.8 Co 0.15 Al 0.05 O 2 and LiNi 0.6 Mn 0.2 Co 0.2 O2 cathodes for 400 and 200 cycles, respectively. Finally, the Li-conducting pathway in the hybrid electrolyte was further investigated by a 6 Li-to- 7 Li isotope replacement method, indicating that Li transport mainly relies on the LLZO and interface between LiBFSIE and LLZO.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strain in Metal Halide Perovskite Thin Films - Interfacial Mechanical Coupling

Hybrid organic−inorganic metal halide perovskites (MHPs) are promising semiconductors for photovoltaics and optoelectronics, but their commercial viability is limited by instability, particularly strain induced by mismatch in coefficients of thermal expansion (CTE) between the perovskite film and substrate. Here, we investigate strain development and relaxation in MHP thin films using in situ bending and Grazing Incidence Wide-Angle X-ray Scattering (GIWAXS). We quantify the film− substrate interfacial mechanical coupling and identify interfacial slippage beyond a critical strain (∼0.4%), with Br-2PACz exhibiting comparatively stronger interfacial mechanical coupling among common interface modifiers. Time-resolved GIWAXS reveals reversible macrostrain during thermal cycling driven by CTE mismatch. Leveraging this behavior, we introduce a prestrain process that induces persistent compressive strain after cooling, with partial relaxation over time. These results provide insight into interfacial mechanical coupling and strain dynamics, offering a framework for strain engineering in perovskite devices.

metals↗

All solid thick oxide cathodes based on low temperature sintering for high energy solid batteries

Solid-state batteries (SSBs) could significantly improve the safety and energy density over conventional liquid cells. One key enabling technology is the use of solid electrolytes. NASICON-type Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) is a very attractive solid-state electrolyte for the cathode side due to its high oxidation potential and high ionic conductivity. The usage, however, is limited by its large interfacial resistance against most of the cathode materials as well as the thermodynamic instability during high temperature sintering needed to achieve high mass density. Here we construct thin, percolative, and mixed conductive interphases through in situ low-melting-point liquid sintering. These mixed conductive interphases drastically improve the kinetics, leading to high-loading solid LATP/LiCoO 2 cathodes achieving capacity loading of up to ~6 mA h cm –2 . The technique is also applicable to Ni-rich cathode materials, achieving up to ~10 mAh cm –2 , which can lead to more than 400 W h kg –1 cells in SSBs. Furthermore, our composite cathodes show a ten-times and three-times area capacity improvement over the state-of-the-art cathodes using oxide and sulfide SSEs, respectively.

25 ENERGY STORAGE↗

Interfacial solvation-structure regulation for stable Li metal anode by a desolvation coating technique

Rechargeable lithium (Li) metal batteries face challenges in achieving stable cycling due to the instability of the solid electrolyte interphase (SEI). The Li-ion solvation structure and its desolvation process are crucial for the formation of a stable SEI on Li metal anodes and improving Li plating/stripping kinetics. This research introduces an interfacial desolvation coating technique to actively modulate the Li-ion solvation structure at the Li metal interface and regulate the participation of the electrolyte solvent in SEI formation. Through experimental investigations conducted using a carbonate electrolyte with limited compatibility to Li metal, the optimized desolvation coating layer, composed of 12-crown-4 ether-modified silica materials, selectively displaces strongly coordinating solvents while simultaneously enriching weakly coordinating fluorinated solvents at the Li metal/electrolyte interface. This selective desolvation and enrichment effect reduce solvent participation to SEI and thus facilitate the formation of a LiF-dominant SEI with greatly reduced organic species on the Li metal surface, as conclusively verified through various characterization techniques including XPS, quantitative NMR, operando NMR, cryo-TEM, EELS, and EDS. The interfacial desolvation coating technique enables excellent rate cycling stability (i.e., 1C) of the Li metal anode and prolonged cycling life of the Li||LiCoO 2 pouch cell in the conventional carbonate electrolyte (E/C 2.6 g/Ah), with 80% capacity retention after 333 cycles.

42 ENGINEERING↗

Electroconvection near an ion-selective surface with Butler–Volmer kinetics

We study the effects of interfacial kinetics on the electro-hydrodynamics of ion transport near an ion-selective surface using a combination of linear stability analysis and numerical simulation. The finite kinetics of the electrolyte–electrode interface affects the ion transfer and electroconvection in many ways. On a surface of fixed topography, such as a metal surface of slow and stable ion deposition or covered by a polymer membrane, the finite kinetics reduces the current in one-dimensional ion diffusion/migration, increases the critical voltage for the onset of the electroconvective instability, changes the dynamics of the electroconvection and the overlimiting current, and enhances the lateral ion diffusion within the interfacial layer. The first three effects are indirectly caused by the reaction kinetics and can be characterized by an effective voltage difference across the liquid electrolyte. In comparison, the last effect is controlled by a direct interplay between kinetics and nonlinear electroconvection. Scaling laws for ion transport and features of electroconvection are proposed. We also analyse the linear stability of a surface which evolves under ion deposition and find that the finite kinetics decreases the growth rate of both electroconvective and morphological instabilities and therefore modifies the wavenumber of the most unstable mode.

Mechanics↗

Low-cost, Highly Efficient and Fast Thermally Pressed Scalable Carbon-based Planar Perovskite Solar Cells

This Final Technical Report summarizes work completed under Award Number DEEE0009833, titled "Low-cost, Highly Efficient and Fast Thermally Pressed Scalable Carbon-based Planar Perovskite Solar Cells." The project addressed the central technical problem that carbon-electrode perovskite solar cells (C-PSCs) can reduce electrode costs and improve environmental durability, but they have historically lagged noble-metalcontact devices due to poor carbon/perovskite contact, high carbon-electrode resistance, imperfect hole extraction, and insufficient operational stability. The Statement of Project Objectives (SOPO), therefore, required systematic engineering of thermally pressed carbon-based planar perovskite solar cells by improving the carbon/perovskite interface quality, improving carbon-electrode conductivity, and further increasing device stability. The work advanced understanding of carbon-based perovskite photovoltaics by connecting device performance to three coupled mechanisms: interfacial recombination at the perovskite/hole-transport-layer/carbon stack; lateral and vertical transport losses in carbon contacts; and instability driven by moisture, heat, illumination, ion migration, and slow/variable manufacturing steps.

14 SOLAR ENERGY↗

A Finite Element Method for Compressible and Turbulent Multiphase Flow Instabilities with Heat Transfer

We present a new finite element framework for modeling compressible, turbulent multiphase flows with heat transfer. For two-fluid systems with a free surface, the Volume of Fluid (VOF) method is implemented without the need for interface reconstruction, while turbulence is resolved using a dynamic Vreman large eddy simulation (LES) model. Unlike most two-phase VOF studies, which neglect heat transfer, the present approach incorporates energy transport equations within the VOF formulation to account for heat exchange, an effect particularly important in turbulent flows. Conjugate heat transfer is often challenging in finite volume methods, which require explicit specification of heat fluxes at the solid–fluid interface, limiting accuracy and predictive capability. By contrast, the finite element formulation does not require heat flux inputs, allowing more accurate and robust simulation of heat transfer between solids and fluids. The method is demonstrated through three representative cases. First, a two-fluid instability with a single-mode perturbation is simulated and validated against analytical growth rates. Second, conjugate heat transfer is examined in a high-temperature flow over a cold metal cylinder, with validation performed both quantitatively—via pressure coefficient comparisons with experimental data—and qualitatively using vector field topology. Finally, compressible spray injection and breakup are modeled, demonstrating the ability of the framework to capture interfacial dynamics and atomization under turbulent, high-speed conditions. In the compressible spray injection and breakup case, the results indicate that the finite element formulation achieved higher predictive accuracy and robustness than the finite-volume method. With the same mesh resolution, the FEM reduced the root mean square error (RMSE) and mean absolute percentage error (MAPE) from 6.96 mm and 26.0% (for the FVM) to 4.85 mm and 12.7%, respectively, demonstrating improved accuracy and robustness in capturing interfacial dynamics and heat transfer. The study also introduced vector field topology to visualize and interpret coherent flow structures and instabilities, offering insights beyond conventional scalar-field analyses.

97 MATHEMATICS AND COMPUTING↗

An Oxygen‐Scavenger Sulfide Coating Enabling Long‐Term Stable Nickel‐Rich Cathodes

Oxygen release is a major issue associated with layer-structured metal oxide cathodes in lithium batteries, which can further cause a series of problems, such as irreversible phase transition, microcracking, and electrolyte decomposition. Eventually, these issues jointly result in cell performance degradation and safety hazards. Thus, it is very significant to tackle oxygen release for achieving long-term stable cyclability, but very challenging. Although intensive efforts have been invested to date, there still lacks a feasible solution. In this study, nanoscale ZrS 2 coatings are applied on prefabricated LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes directly via atomic layer deposition (ALD). Very encouragingly, we reveal that this ALD-deposited conformal ZrS 2 nanocoating can serve as an exceptional oxygen scavenger and then convert into a stable sulfate (Zr(SO 4 ) 2 ) coating. Such an in situ conversion is very beneficial and effective for protecting the electrolyte from decomposition. In addition, the resultant Zr(SO 4 ) 2 coating further inhibits undesirable reactions, stabilizes the interface between NMC811 and the electrolyte, suppresses microcracking, mitigates transition metal dissolution, and maintains the structural stability of the NMC811 cathode. Consequently, the ZrS 2 -coated NMC811 cathode has demonstrated extraordinary performance. Thus, this study advances the understanding of interface engineering while paving a new technical pathway for commercializing NMC811 cathodes.

Nickel-rich cathodes↗

Atomic-scale constituting stable interface for improved LiNi 0.6 Mn 0.2 Co 0.2 O 2 cathodes of lithium-ion batteries

Ascribed to their higher capacity and lower cost compared to conventional LiCoO 2 , the Ni-rich layered LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC622) is now considered as one promising cathode for lithium-ion batteries (LIBs). However, it still suffers from some evident performance degradation, especially under high cutoff voltages (i.e., >4.3 V versus Li/Li + ). The performance degradation typically is exhibited as capacity fading and voltage drop, mainly originating from an instable interface between the NMC622 and electrolyte as well as the evolution of the NMC structure. To improve the interfacial and structural stability of NMC cathodes, herein we deposited an ultrathin layer of Al 2 O 3 coatings (<5 nm) conformally over NMC622 composite electrodes directly using atomic layer deposition (ALD). It was found that, under different upper cutoff voltages (4.3, 4.5, and 4.7 V), the ALD Al 2 O 3 coatings enable enhanced performance of NMC622 cathodes with better cyclability and higher capacity. Particularly, the beneficial effects of the ALD Al 2 O 3 coatings are more remarkable at higher upper cutoff voltages (4.5 and 4.7 V). Furthermore, the ALD coatings can significantly improve the rate capability of NMC622. To this end, we utilized a suite of characterization tools and performed a series of electrochemical tests to clarify the effects of the ALD Al 2 O 3 coatings. This study revealed that the beneficial effects of the Al 2 O 3 ALD coatings are multiple: (i) serving as an artificial layer of solid electrolyte interphase to mitigate undesirable interfacial reactions; (ii) acting as a physical barrier to inhibit metal dissolution of NMC; and (iii) forming a reinforced networked overcoating to boost the mechanical integrity of NMC cathodes. This study is favorable for designing high-performance NMC cathodes.

25 ENERGY STORAGE↗

Conformally coated scaffold design using water-tolerant Pr 1.8 Ba 0.2 NiO 4.1 for protonic ceramic electrochemical cells with 5,000-h electrolysis stability

Protonic ceramic electrochemical cells (PCECs) have potential as long-duration energy storage systems. However, their operational stability is limited under industrially relevant conditions due to the intrinsic chemical instability of doped barium cerate-based electrolytes and oxygen electrodes against H 2 O, as well as the poor electrode–electrolyte interfacial contact. Here, in this study, we present a conformally coated scaffold (CCS) design to comprehensively address these issues. A porous proton-conducting scaffold is constructed and conformally coated with Pr 1.8 Ba 0.2 NiO 4.1 electrocatalyst, which has high chemical stability against H 2 O, triple conductivity and hydration capability, and protects vulnerable electrolytes from H 2 O. The CCS structure consolidates the electrode–electrolyte interfacial bonding to enable fast proton transfer in the percolated network. This design enables PCECs to reach electrolysis stability for 5,000 h at −1.5 A cm−2 and 600 °C in 40% H 2 O. This work provides a general strategy to stabilize PCECs and offers guidance for designing resilient and stable solid-state energy storage systems.

Protonic ceramic electrochemical cell↗

Ultrathin stable Ohmic contacts for high-temperature operation of β -Ga2O3 devices

Beta gallium oxide (β-Ga2O3) shows significant promise in high-temperature, high-power, and sensing electronics applications. However, long-term stable metallization layers for Ohmic contacts at high temperatures present unique thermodynamic challenges. The current most common Ohmic contact design based on 20 nm of Ti has been repeatedly demonstrated to fail at even moderately elevated temperatures (300–400 °C) due to a combination of nonstoichiometric Ti/Ga2O3 interfacial reactions and kinetically favored Ti diffusion processes. Here, we demonstrate stable Ohmic contacts for Ga2O3 devices operating up to 500–600 °C using ultrathin Ti layers with a self-limiting interfacial reaction. The ultrathin Ti layer in the 5 nm Ti/100 nm Au contact stack is designed to fully oxidize while forming an Ohmic contact, thereby limiting both thermodynamic and kinetic instability. This novel contact design strategy results in an epitaxial conductive anatase titanium oxide interface layer that enables low-resistance Ohmic contacts that are stable both under long-term continuous operation (>500 h) at 600 °C in vacuum (≤10−4 Torr), as well as after repeated thermal cycling (15 times) between room temperature and 550 °C in flowing N2. This stable Ohmic contact design will accelerate the development of high-temperature devices by enabling research focus to shift toward rectifying interfaces and other interfacial layers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗